Process of and apparatus for dissolving radium emanation in fluids



' 1,6`5,1 July 5,` 1927. A'CERVI 3 13 PROCESS 0F AND APPARATUS FOR DIsSoLvING RADIUM EMANATION IN FLUIDS Filed March 16, 1926 Figi.

2 Sheets-Sheet 1 A Troie/VER 35. 55' n uy 51921 ACERW l 1,635,113

PROCESS OF AND APPARATUS FOR DISSOLVING RADIM EMANATION IN FLUIDS Filed March 16, 1926 2 Sheets-Sheet 2 '11114lllllllllllll'lrllllln 'lll ATTO/wv@ y Patented July 5, 1927.

UN-rrEfD siAra-s rATENT orifice.-

ARMANDO oEnvI, or NEW YORK, n. Y., Assisiion To "rien minion ivIAiiArioii oonroRATroN, or NEW Yoan, ii. Y.,

A CORPORATION OF DELAWARE.

rfaoonss or AND ArrAnATUs non nissonirire RADUM nfMANArioir 1N rilni'ns.

Application filed March 16, 1926. Serial No. 95,119.

internal1 use Without allowing the `radium eimaiiation to` escape from solution and this `is accomplished by preventing the activated liquidA or solutioii,`from coming in `contact with the atmosphere.

i The iragileHseeds referred to cont-ain lradium emanationlin equilibriuurwith the products `of decompositionot radium emanatjion. yTheradium,emanation itself is a decay `product. of radium; itl is a and it collects above a solution oi' radium for ex-" ample radium bromide. Then using a radium bromide solution, the impure emanatioii may be purified by substantially com- .pletely removing the impuritieswhich in the major portion comprise, hydrogen chloride, hydrogen bromide, Water vapor, hy-

drogen,

andhydrogen peroirid` Any suitable purification mediums may be employed .but l prefer to treat the impure emanation ias follows:

The gas is v passed through potassium hydroXid, then through a heated cupricj and cuprous oxidcoil and iinally th rough phosphorousy pentoxid.

Radium emanation is a gas and is the iirst disintegration. product of radium. It occurs `in nature as a .gas or in` solution in Waters that have passed through uranium and radium deposits.

The spring ivaters containing radium emanatfon in solution,

suoli ast atoga, et

hose of Carlsbad, Joachimstal,` Sarc., have been found beneficial when Heretotore, to obtain by artificial means, a solution of radium einanat-ion in Water, the procedure haspbeen as follows: Air was buttata through an `acid aqueous solution ot radium bromide and radium chloride. The resulting; mixture of air and radium emanation iras then passed through 'an allraline b ture iva tnfnes1 ath and the purifiedgaseous mixs bubbled through water several The Water absorbed the radium emanation and was thenreadydfor drinking purposes. The Vabsorption ot ,the radium emanation occurs in a bottle having'an open top. Y Theabove,procedure is .objectionable as 55 will appear from the follvoivinfr:

(l) `The solution contains amounts otradiuin varying from 1/2 mg. to 2 mg., the maximum amount of radium enianat-iOnbeing given oit by the radium solution,each` day being, at best, 0.33 millicuries of emanatioii, Lai-ger amountsfare only possible-by having more radium in solution; This is impractical because of the high price of radium. v i

(2) Since the amount of radium emanation given otl' each day is very small, the efficiency of the process is very much impaired because the emanation is passed through tivoditlierent solutions.`

is always mixed with the emanation.v 4Although the absorption 'of the radium emanation is not affected by the partialpressure of the gases mixed With it, `as proved by Boyle, the volume o'tair is such that a large amount ot radium einanation Will remain undissolved, as proven below.

(5)' The bottle containing the radium enia'nation solution has an open top so that the emanation easily escapes from solution, aspr'oven below. l

The statements of :paragraphs t and 5 depend for their accuracy on the following:

The coetlicient of absorption o'ffradium eiiianatioirin Water is 0.25. It is 1defined as iolloWs:-[t a certain mixture of air` and radium emanation of volume V1 is enclosed in a closed container. of volume V partially filled with Water of'volumey2` so that vvff'l-VlgzV; and the containerlis shaken so as to allow the einanation to come in intimate contact with the Water, then it Elthe amount of radium emanation in gas E2=the amount oit radium emanation in the 2. i i' l 1,635,113

liquid, the radium emanation will be ab-V in liquid V :thet-oiiceiitration ol radium .l l 1 l emanatioiiin the'gas. l'ii'hen equilibrium reaehedjf and will have delinite values and at constant temperature and. pressure,

gl=aa constant i "1 1,2 i i i' v1 This-constant, a, is called the coefficient of,

absorption of radium emanation bythe liquid. Starting with a delinite `amount of and call E 2l, the following results since at room temperature @51025.

To obtain complete` vabsorption of the radium emanation by the liquid, E (the total amount ofi'adium `emanation started with) `must be made equal to E2 (amount of the radium emanation absorbed) "as shown by formula II; This can only be accomplished by making V, `(volume oil Athe `iras) substantially negligible which cannot be accomplished with the apparatus previously described.

It isevident li'iom the above, that if air is circulated through a. radium solution, and

`this air is passed throughtlie Waterto be activated, that whatever air is used, is going' to take much olf the radium' emanatioii; and further, When the (glass containing theY water is .disconnected irom the apparatus for drinkingr the activatil wateiglhe surface oli the water will be exposed to the atmosphere thereby making V, suddenly equal to inlinity, the result being'` that the radium emanation` Ain solution tends to escape int-o `the atmosphere.

According' to my invention, the Water sub stantially completely absorbs all the radium emanation used. This is accomplished;Erst, by` usingr only purified" radium emanation which has a very small volume, for example, about 1/2 c. nim.; second, by havingr a large amount of Water pass through the compartment Where the radium emanation --=the concentration of radium emanation` is en-` closed; and third, by preventing; the ac tivated'solution containing radium eiiianation from coming in contact with the` atmosphere. Since thev fragile `,:upillary tubes previously referred to may contain radium emanation in nany desired` eoncentiutioii, it isseen that accoriling to niyiinvciiti-on, the use of radium itself dispensed with. lii'oadly` stated7 myinvention `consists= in a process of -p reparing' l'or internal administration` an activated fluid such as an aqueous solution comprii'siiigir bringing the iadiuin emanation into solution and then administering the saine, both the solution step and the administering step occurring?,l iii `the sub- "stantial absence of a diluting fluid, for ci;-

ample, air. f Stated differently, my invention comprises a process el preparing tor iiitei'nal administration an aeilivated lluid con-` tainingr radiiiiiiemanation coml'irisiupI ini tial- `ly bringing'the radium eiiianationinto solution in the absence of a diluting fluid and then preservingthe resulting activateil fluid l from substantial contact with ol lier .fluids uiitil the activated fluid is administered. Further, my invention provides an apparatus lor preparing activated iuids containinpr radium emanation for internal administration comprising' a receptacle having a `fluid such as, for example, w'aterpresent therein to seal the receptacle from the atmosphere, a crushing mechanism lin operative connectionwith said. receptacle, a fragile seed in` said crushing' mechanism having present radium einanation capable ot being liberated on crushing and going into solution inthe fluid, `an administering conduit adapted `to receive the activated. solution and means to positively administer the activated `fluid and prevent the saine from coming in contact with the atmosphere. As will be pointed out, iii detail, this latter means may comprise a water head in combination with an activated pis ton or the equivalent thereof which may consist simply of a hydrostatic head as will be later described in connection with Figure l. It is vto beunderstciod that the radium emanation may be `dissolved in ftheL lluid, either liquid or gases, but,`at the present time, the mostsatisfactorycarrying vehicle is a liquid such as Water.V Of course, liquids other than Water may beused if desired.

In order that my invention maj. be clearly understood reference iis made lo the accompanyiiri,r drawing wherein,

Figure l is a side view partially in section showing the liquid, receptacle, the crusliiiunz: mechanism and the administering conduit all in operative connection.

Figure 2is a longitudinal sectional vieu1` of` the Crusher mechanism.

Figure 2a is a horizontal ceiiti'alsection lthrough vFigure 2.

l lll) IUI) lthe Crusher mechanismtakenon line Svi-3.

gFigure 4 isa side View of the capillary tube before it is broken. 1

Figures and 6 show va capillary tube broken in three pieces and illustrate the trapping of the emanation in the absence of crushing.

Figure 7 is a side view of a modified form .of amaratus wherein an aetivatinff oiston such as water 2, a crushing device ormechanism 3 in operative connection with the 4liquid receptacle 1 by means of conduit 4 and an administering conduit 5. j

` rllhecrusher device comprises a `body tube 6, an inlet member or tube 7 and an activated liquid outlet or tube S. The screw 9 is in operative connection with crushing jaws hereafter to be mentioned in detail. The inlet tube 7 `and the outlet tube 8 are provided `l` `with shoulders 10 and 11 abutting against `the ends of the body tube 6 and held there tightly by caps 12 and 13 provided with bayonet slots 14, 15, 1G and 17 forming bayonet joints with pins 18, 19, and 21. The structure set forth insures a liquid tight bOdy eonnertion between theinlet member or "lube T and the body tube G and the outlet tube tl.

The inlet member 7` is provided with a passage way 22 leading to the crushing compartment In outletmember 8 there is a passage way 24 also leading to thecruslr ing chamber 23. At the end 27 of the inlet passage 22, there is integral therewith a lower stationary jaw 25 provided fwith teeth 26yk the jaw 25, as shown in Fig. 2

' covering a portion of the end 27 of the paslil) way T he remainder of the end portion 27 is covered by a screen 28 of approximately 300 mesh. At the end 29 of the outs passage 24 there is a screen 30 of approximately 300 mesh.

i The crushing screw 9 is provided with a projection 33 carrying a head 34 to which there is removedly secured an upper mow able jaw 31 having teeth 32. The compartment formed by the screens 28 and 30 and the movable and stationary jaws 31 and 25 respectively may be termed the crushing compartment 23. Into this crushing compartment, an emanation seed such as shown in 4 may be charged by removing the cap 35 carrying the rod 35 vfrom the tube .36 se as to enable the charging'of a seed carrying radium emanation into the crushtially completely filling the. passage way 87.

ing compartment 23, 4lt will Vbe observed that the rod 35 substantially iills'the tube passage way 37. This structure `is provided to prevent water from entering the passage way 37 aswhen this occurs the radium emanation is occluded in the water andlthis is not desirable.

The operation of the Crusher' device is follows: A seed containing radium ema-`- nation is inserted through the passage way, 37 j into the crushing compartmentl` `23. Thereafter-the cap 35 carryingv the rbd 35 is put on the tube 36 the rod 35 substan- The cap 35 is tightly held to the tube 36^by means of `the bayonet joint 38. The seed containing radium emanation as it enters the crushing compartment is positionedbetween the stationary aw 25 and the movable `j'aw 31 which is activated by the screw` mem ber 9. Upon bringing the movable jaw 31 closer to the stationary jaw 25 theemanation seed is finely1 crushed liberating the radium emanation which tabsorbed'by the, water filling the crushing chamber 23 lwhereby the water is activated. It isA to be noted thatby crushing the capillary tubes containing radium emanation under water, the emanation'is brought into intimate Contact with thewater; In: this connection. it may be statedthat crushing is absolutely necessary and that mere breaking will net. suffice. The radium emanation in the capillary tube is under a pres-iw. sure of one-half an atmosphere. Ifthe tube 39 shown in Fig. 4 is .broken into `three pieces 40,` 41and 42 as showninA Figs. 5 and 6, the water rushes in in the directionY of the arrowsV and as a result thereof, the` emanation `is trapped `by the water 44 and the solution isV not properly activated. The crushing device set forth operates to finely crush the fragile seed such as a glass seed containing radium emanation and liberate the emanation"without the formation `of radium emanation pockets. The crushing operation is carried `out under' water and in a small compartment of approximate `and 30 approximately 300 or 400 mesh.

These screens function to prevent any pieces of crushed glass from passing through the passage way 24 and the administering 'conduit 5 or through the passage way 22 to the liquid receptacle. 1. The shape of the crushing compartment 23 also tends to prevent the formation of pockets where the radium emanation may be occluded. lVhen the crushing compartment is in operative relation with the administering conduit and a liquid receptacle, containing water, it is appropriate to allow a large volume `of water between 100 and 200 c. e. per minute to flow in one direction through the crushing compartment 23 whereby the pieces `of broken glass will be Washed and the radium einanation repeatedly presented with fresh Water and in this Way the fresh Water is made to pass `constantly through and aby sorb the radium emanation present. This method of procedure approximates ideal extracting coni'litious and aft the saine time `ideal means; since all the water comes in Contact with substai'itially all ot the broken pieces of The process as carried out in the appa- `ratus shown prevents the charged Water `from coming in contact with the atmosphere .and'tliercby eliminates the escape of the `radium` einanation into the atmosphere.

`This may beV accomplished by employing any of the following; y

(1) `There may be a unidirectional tloiv` .of the `water from the liquid receptacle into the crushing compartment 23 and then directly into themouth piece.

(2) Instead of employing a unidirectional flow off Water acirculatorial system may be providedythatiis, a flow in two direction as will be noted from an examination ot F ig.

i 7 This maybe varied by providing a flow in two directions and having the Water level protected with a' layer of liquid lighter than Water `and immiscible with Water. Various types liquid immiscible With Water may `beused but light mineral oil is preferred. (3) -The Crusher arrangement, the liquid receptacle, `and the administering conduit may all be integral as shown in Fig.` 8.

Referring to Fig. l, it Will 'be noted that `thecrusher device 3 is connected through the outlet 8 withthe administering conduit 5 by means of the flexible tube 5L which may be of rubber. ne'ctedto the conduit 4, preferably inadeo'f rubber.

The inlet conduit 7` is con- The container 1-maybe of any preifeiiedsize but, it is `convenient to have #as tube i `the crushing `coinpartiuent 23 through the thevoluine thereof approximately 200 c. c.

i When the crushing operation iscarried out,

passage Way or tube 8 and the administering conduit It `is noted that the level of the "Water in the liquid receptacle which Will be the same as in the administering conduit 5. After the apfifiaratus has been flooded with water descrilgied, the glass tube which has been inserted into the crushing compartment 23 is crushed `by operation of the screw member 9 and movable crusher'iawl. After the crushing has taken place, the `movable jaw 25 is separated from the stationary jaw 31.,"l`hernouth ol a person is then applied to the adii'iinistering conduit 5 and liquid container l is raisedl from six to twenty niches. thereby orcingthe water in the liquid container or receptacle l through the crushing compartment Q3 of the Crusher device 3, the administering Aconduitti and thereby7 directly into tlieymouth of the person. `Proceeding`-` as set forth, theactivated solution containing radiumemanation iinijiregiiated therein is preserved from substaiitial Contact Witli'othertiuids until the activated solution is administered. A

The apparatus `for preparing an activated' .liquid containing radium emanation and administering the samedirectly is preferably that shown in Fig. l because of they simplicity and ciiiciency of the` apparatus. It is to benoed thatatter the glass" capillary tube containing radium emanation has been crushed under Water in the crushing eoiiunirtmcnt Q?) of the Crusher device 3 the radiiiin cn'ianation will. tend `to dissolve in the Watersui-rounding it and thereby diffuse iii all directions. the direction ot the administering conduit 5, since in that direction the solution leads to the n'iouth ot.' the person to be treated." Ditlfusion in the direction ot the liquid `recep-` tacle l is not desirablefsince the watercoutained therein isfopen to the atmosphere. However, upon `raising the liquid receptacle l1 Vthe water flows from' this receptacle into the crushing compartment 2301i the crusher device 3 at a greater speed than` the `speed of diffusion ofthe radium emanation solu tion intheopposite direction. ln this manfner, the radium `enriauatitui solution is never inycoutaet ivitli theatinospherc and `there-n fore, the radium emanation does not escape.

Referring to Fig. T, the-.liquid receptacle is `provided with a pistont fitting water tightiandhaving an outlet conduit 47 pro` vided with astop cock /l-S. The crusher inechanisiii 3 is in operative connection by means of the inlet member 7 `with the liquid container elfi. '.lhe outletA member 8 of the ci'usher mechanism 3 is in operative connection With y the administering conduit 49 which When solution is not being administered dips into the water F0 in the receptacle 51.

With the liquid receptacle 45 empty and the liquid'receptacle 5l partly full ofwater,

the capillary `tube containing radium` emanation is charged into the Crusher device 3 with the jaws of the crusher device as tar as possible, crushing occurring later.` The `piston 47 is then brought all theway down 9 Diffusion is desirable in` water.V With the stop cock` 48'closed, the` piston 47 is raised slowly drawing water from the liquid receptacle 5l into the liquid container 45. The air originally contained in the crushing Vmechanism is drawn i' along with the water. The stop cock 48 is then opened and the piston'47 Vpushed down therej by forcing out all the air above the water level of the water 52 contained in liquid receptacle 45. The flow of water `from the outlet 47 is an indication of absence'of air inthe cylindrical' liquid receptacle 45. The stop coclr 4S is then closed. At this stage of the operation, the crushing compartment 23 of the crusher device 3 is full of water and there is some water in the cylindrical liquid receptacle with absolutelyv no air in the system. The fragile capillary tube containing the radium emanation'is then crushed by bringing together the jaws of the crushing mechanism. These jaws are then immediately separated.

Thereafter the piston 4G is raised Islowly until the cylindrical receptacle 45 is full of solution, the yincoming' fresh water having washed the broken pieces of glass and the radium emanation present'. The adminis* tering tube 49 is then turned up and applied directly tothe mouth of the `person who wishes to drink the solution. 46 is pressed down by means of the piston rod 53 thereby forcing the solution through the crushing compartment 23 and directly into the mouth of the person. In this man ner the glass pieces are washed twice, once by fresh water and then by charged water.

Referring to Figure 8, 54 is a cylindrical liquid receptacle provided with a piston 55 having a` piston rod 5G, a piston forming a water tight connection with the liquid receptacle 54. The piston 55 carries an outlet administering tube 57 which is preferably made of glass. This administering conduit 57 carries a fine screen 58 approximating 300 mesh. The lower portion of the container 54 is provided with a crushing device comprising a stationary jaw 59 and a movable jaw 60 operated by the screw member 6l. In pperation, the piston 55 is entirely removed from the liquid receptacle 54, the crushing jaw 60 is separated from stationary jaw 59 by means of' screw 61 and a glass tube containing radium emanation is placed between the crushing jaws 59 and GO respectively. Thereafter, the screw 6l is turned until the fragile tube containing the radium einanation is held between the jaws 59 and 60 and is not broken thereby. The

liquid receptacle 54 is then filled with water i and piston 55 is placed into the .receptacle 54 and pushed down until a portion of the The piston water 62 showsinto the mouth administer-- ing conduit. 57 .f vThis indicates the absence of air from the liquid receptacle 5 4. VThen,A the emanation tube is crushed byv advancing the movable jaw. 6() as far as it. will go. Theinovable jaw 60 is then withdrawn by means of the screwl and the radium Veinanation is thereby enabled to come iii-con# tact with'the water; A persons mouth isapplied` directly through the administeringA conduit 57 and piston 55 is pushed by the pistonv rod 56 all the way in thereby forcing the activated liquid intothe mouth of `the person without Vallowing the activated liq uid to come incontact with the atmosphere;V

If desirable screens having awpproximatelyQ 400 mesh may be used insteadof those hav# ing 300 mesh.

Radium emanation solutions andrespecially those prepared in the absence ofdi luting fluids may also be effectually admin istered byintravenous injection of the solution, and this may be accomplishedby using a hypodermic needle instead of a m'buth piece. i i

`The crusher mechanism above described forms the subject matter of myVco-p'ending application which has become Patent 1,614,-V S25. i 11 I claim: V Y i t 1..T he .process of preparing-for internal administration, an activatedl fluidcarrying' radium emanation comprising? initiallyl bringing the radium emanation int-o s0lu` tion in lthe absence of ay diluting.. fluid, and preserving the resultingactivated solution! from substantial contact with other fluids until the activated solution is administered.

2. The process of preparing for internal administration, an activated fluid carrying radium emanation comprising initially bringing-the radium emanation into solution in the absence of a diluting fluid, and preserving the resulting activated solution from substantial contact with the atmosphere until the activated solution is administered.

3. The process of preparing for internal administration, an activated fluid carrying radium emanation comprising crushing a fragile seed containing radium einanation in the presence of the carrying vehicle, the crushing step being carried out in the substantial absence of a diluting fluid, and preserving the resulting activated fluid in .the substantial absence of a diluting iiuid until administered.

4. The process of preparing for internal administration, an activated fluid carrying radium emanation comprising crushing a fragile seed containing radium emanation in the presence of a carrying vehicle and in the substantial absence of a diluting fluid.

5. The process of preparing for internal administration, an activated fluid carrying radium emanation comprising crushing a llt) fragile seed containing radium emanation in the presence of 4an aqueous carrying vehicle and in the substantial absence of air.

6. The process of preparing forza-internal administration, an activated solution carrying` radium emanation comprising charging a ragile seed containing radium einanation into a crushinor compartment which is in connection rWiti li uid,` filling said crushing compartment with liquid drawn from said receptacle, allowing tlie liquid to pass into an administering conduit until the level of the Water in the administering conduit is the same as that in the liquid receptacle, and then crushing the fragile sed to liberate "the Aradium manation and activate Vthe liquid. A y

`7An` activated liquid carrying radium emanation impregnated therein in which diluting fiuids are substantially absent. n

8. An: activated `liquid-carrying radium a enianation` impregnated therein in 4 which 1 diluting gases are substantially absent.

9. An activated liquid carrying radium n emanation impregnated therein in which air is substantially absent.

. 10.` An activated.aqueous solution carrying radium einanation impregnated therein in which air is substantially absent-` H11. Apparatus for preparing `activated fluids containing radium emanation forinternal administration comprising a receptacle having a fluid present to seal the rece tacle` from the atmosphere, a crushing' mec anism in operative connection Withsaid a receptacle containing rece tacle, Aa fragile seed "said lern-Shing; I

mec ianism having present radium emanation capable of being liberated on crushing, and going into solutionin the fluid, an` administering conduitadapted to receive the activated :solution and means to ositively administer the activated fluid and, prevent the same from coming in contact With the atmosphere.

12. Apparatus fluids containing radium emanation for internal administration comprising a receptacle having a fluid present to seal the receptacle from the atmosphere7 a crushing mechanism in operativeiconnection with saidrece tacle, a `fragile seed in said crushing mec anism liavin' .present radium emanation capable of being liberated on crushing,fand goin into solution in the fluid, an administering conduit adapted to a ARMANDO cERvI.

forV preparing activated, 

